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Bagotsky V.S. Fuel Cells.. Problems and Solutions (Wiley, 2009 FUEL CELLS Problems and Solutions VLADIMIR S. BAGOTSKY A.N. Frumkin Institute of Electrochemistry and Physical Chemistry Russian Academy of Sciences Moscow, Russia FUEL CELLS FUEL CELLS Problems and Solutions VLADIMIR S. BAGOTSKY A.N. Frumkin Institute of Electrochemistry and Physical Chemistry Russian Academy of Sciences Moscow, Russia Copyright r 2009 by John Wiley & Sons, Inc. All rights reserved. Published by John Wiley & Sons, Inc., Hoboken, New Jersey. Published simultaneously in Canada. No part of this publication may be reproduced, stored in a retrieval system, or transmitted in any form or by any means, electronic, mechanical, photocopying, recording, scanning, or otherwise, except as permitted under Section 107 or 108 of the 1976 United States Copyright Act, without either the prior written permission of the Publisher, or authorization through payment of the appropriate per-copy fee to the Copyright Clearance Center, Inc., 222 Rosewood Drive, Danvers, MA 01923, (978) 750-8400, fax (978) 750-4470, or on the web at www.copyright.com. Requests to the Publisher for permission should be addressed to the Permissions Department, John Wiley & Sons, Inc., 111 River Street, Hoboken, NJ 07030, (201) 748-6011, fax (201) 748-6008, or online at http://www.wiley.com/go/permission. Limit of Liability/Disclaimer of Warranty: While the publisher and author have used their best efforts in preparing this book, they make no representations or warranties with respect to the accuracy or completeness of the contents of this book and specifically disclaim any implied warranties of merchantability or fitness for a particular purpose. No warranty may be created or extended by sales representatives or written sales materials. The advice and strategies contained herein may not be suitable for your situation. You should consult with a professional where appropriate. Neither the publisher nor author shall be liable for any loss of profit or any other commercial damages, including but not limited to special, incidental, consequential, or other damages. For general information on our other products and services or for technical support, please contact our Customer Care Department within the United States at (800) 762-2974, outside the United States at (317) 572-3993 or fax (317) 572-4002. Wiley also publishes its books in a variety of electronic formats. Some content that appears in print may not be available in electronic formats. For more information about Wiley products, visit our web site at www.wiley.com. Library of Congress Cataloging-in-Publication Data: Bagotsky, V. S. (Vladimir Sergeevich) Fuel cells: problems and solutions/Vladimir Bagotsky p. cm. Includes index. ISBN 978-0-470-23289-7 (cloth) 1. Fuel cells. I. Title. TK2931.B35 2008 621.31u2429–dc22 2008033276 Printed in the United States of America 10987654321 CONTENTS PREFACE xi SYMBOLS xiii ACRONYMS AND ABBREVIATIONS xv I INTRODUCTION 1 INTRODUCTION 3 1 THE WORKING PRINCIPLES OF A FUEL CELL 7 1.1 Thermodynamic Aspects 7 1.2 Schematic Layout of Fuel Cell Units 11 1.3 Types of Fuel Cells 15 1.4 Layout of a Real Fuel Cell: The Hydrogen–Oxygen Fuel Cell with Liquid Electrolyte 15 1.5 Basic Parameters of Fuel Cells 20 Reference 26 2 THE LONG HISTORY OF FUEL CELLS 27 2.1 The Period Prior to 1894 27 2.2 The Period from 1894 to 1960 30 v vi CONTENTS 2.3 The Period from 1960 to the 1990s 33 2.4 The Period After the 1990s 39 References 40 II MAJOR TYPES OF FUEL CELLS 43 3 PROTON-EXCHANGE MEMBRANE FUEL CELLS 45 3.1 History of the PEMFC 46 3.2 Standard PEMFC Version from the 1990s 49 3.3 Special Features of PEMFC Operation 54 3.4 Platinum Catalyst Poisoning by Traces of CO in the Hydrogen 57 3.5 Commercial Activities in Relation to PEMFCs 59 3.6 Future Development of PEMFCs 60 3.7 Elevated-Temperature PEMFCs 67 References 70 4 DIRECT LIQUID FUEL CELLS 73 PART A: DIRECT METHANOL FUEL CELLS 73 4.1 Methanol as a Fuel for Fuel Cells 73 4.2 Current-Producing Reactions and Thermodynamic Parameters 74 4.3 Anodic Oxidation of Methanol 74 4.4 Milestones in DMFC Development 76 4.5 Membrane Penetration by Methanol (Methanol Crossover) 77 4.6 Varieties of DMFCs 79 4.7 Special Operating Features of DMFCs 81 4.8 Practical Models of DMFCs and Their Features 83 4.9 Problems To Be Solved in Future DMFCs 85 PART B: DIRECT LIQUID FUEL CELLS 87 4.10 The Problem of Replacing Methanol 87 4.11 Fuel Cells Using Organic Liquids as Fuels 88 4.12 Fuel Cells Using Inorganic Liquids as Fuels 94 References 97 CONTENTS vii 5 PHOSPHORIC ACID FUEL CELLS 101 5.1 Early Work on Phosphoric Acid Fuel Cells 101 5.2 Special Features of Aqueous Phosphoric Acid Solutions 102 5.3 Construction of PAFCs 103 5.4 Commercial Production of PAFCs 104 5.5 Development of Large Stationary Power Plants 105 5.6 The Future of PAFCs 105 5.7 Importance of PAFCs for Fuel Cell Development 107 References 107 6 ALKALINE FUEL CELLS 109 6.1 Hydrogen–Oxygen AFCs 110 6.2 Alkaline Hydrazine Fuel Cells 117 6.3 Anion-Exchange (Hydroxyl Ion–Conducting) Membranes 121 6.4 Methanol Fuel Cells with Anion-Exchange Membranes 122 6.5 Methanol Fuel Cell with an Invariant Alkaline Electrolyte 123 References 123 7 MOLTEN CARBONATE FUEL CELLS 125 7.1 Special Features of High-Temperature Fuel Cells 125 7.2 Structure of Hydrogen–Oxygen MCFCs 126 7.3 MCFCs with Internal Fuel Reforming 128 7.4 Development of MCFC Work 130 7.5 The Lifetime of MCFCs 131 References 133 8 SOLID-OXIDE FUEL CELLS 135 8.1 Schematic Design of Conventional SOFCs 136 8.2 Tubular SOFCs 138 8.3 Planar SOFCs 143 8.4 Monolithic SOFCs 146 8.5 Varieties of SOFCs 147 8.6 Utilization of Natural Fuels in SOFCs 149 8.7 Interim-Temperature SOFCs 151 8.8 Low-Temperature SOFCs 155 8.9 Factors Influencing the Lifetime of SOFCs 157 References 158 viii CONTENTS 9 OTHER TYPES OF FUEL CELLS 161 9.1 Redox Flow Cells 161 9.2 Biological Fuel Cells 164 9.3 Semi-Fuel Cells 167 9.4 Direct Carbon Fuel Cells 170 References 174 10 FUEL CELLS AND ELECTROLYSIS PROCESSES 177 10.1 Water Electrolysis 177 10.2 Chlor-Alkali Electrolysis 182 10.3 Electrochemical Synthesis Reactions 185 References 187 III INHERENT SCIENTIFIC AND ENGINEERING PROBLEMS 189 11 FUEL MANAGEMENT 191 11.1 Reforming of Natural Fuels 192 11.2 Production of Hydrogen for Autonomous Power Plants 196 11.3 Purification of Technical Hydrogen 199 11.4 Hydrogen Transport and Storage 202 References 205 12 ELECTROCATALYSIS 207 12.1 Fundamentals of Electrocatalysis 207 12.2 Putting Platinum Catalysts on the Electrodes 211 12.3 Supports for Platinum Catalysts 214 12.4 Platinum Alloys and Composites as Catalysts for Anodes 217 12.5 Nonplatinum Catalysts for Fuel Cell Anodes 219 12.6 Electrocatalysis of the Oxygen Reduction Reaction 221 12.7 The Stability of Electrocatalysts 227 References 228 13 MEMBRANES 231 13.1 Fuel Cell–Related Membrane Problems 232 13.2 Work to Overcome Degradation of Nafion Membranes 233 CONTENTS ix 13.3 Modification of Nafion Membranes 233 13.4 Membranes Made from Polymers Without Fluorine 235 13.5 Membranes Made from Other Materials 237 13.6 Matrix-Type Membranes 237 13.7 Membranes with Hydroxyl Ion Conduction 238 References 239 14 SMALL FUEL CELLS FOR PORTABLE DEVICES 241 14.1 Special Operating Features of Mini-Fuel Cells 242 14.2 Flat Miniature Fuel Batteries 243 14.3 Silicon-Based Mini-Fuel Cells 245 14.4 PCB-Based Mini-Fuel Cells 247 14.5 Mini-Solid Oxide Fuel Cells 248 14.6 The Problem of Air-Breathing Cathodes 249 14.7 Prototypes of Power Units with Mini-Fuel Cells 250 14.8 Concluding Remarks 253 References 253 15 MATHEMATICAL MODELING OF FUEL CELLS 255 Felix N. Bu¨chi 15.1 Zero-Dimensional Models 257 15.2 One-Dimensional Models 257 15.3 Two-Dimensional Models 258 15.4 Three-Dimensional Models 259 15.5 Concluding Remarks 260 References 260 IV COMMERCIALIZATION OF FUEL CELLS 263 16 APPLICATIONS 265 16.1 Large Stationary Power Plants 265 16.2 Small Stationary Power Units 269 16.3 Fuel Cells for Transport Applications 272 16.4 Portables 277 16.5 Military Applications 281 References 283 x CONTENTS 17 FUEL CELL WORK IN VARIOUS COUNTRIES 285 17.1 Driving Forces for Fuel Cell Work 285 17.2 Fuel Cells and the Hydrogen Economy 287 17.3 Activities in North America 289 17.4 Activities in Europe 290 17.5 Activities in Other Countries 291 17.6 The Volume of Published Fuel Cell Work 294 17.7 Legislation and Standardization in the Field of Fuel Cells 295 References 296 18 OUTLOOK 297 18.1 Periods of Alternating Hope and Disappointment 297 18.2 Some Misconceptions 299 Klaus Mu¨ller 18.3 Ideal Fuel Cells 300 18.4 Projected Future of Fuel Cells 302 References 304 GENERAL BIBLIOGRAPHY 305 AUTHOR INDEX 309 SUBJECT INDEX 315 PREFACE When fuel cells were first suggested and discussed, in the nineteenth century, it was firmly hoped that distinctly higher efficiencies could be attained with them when converting the chemical energy of natural fuels to electric power. Now that the world supply of fossil fuels is seen to be finite, this hope turns into a need: into a question of maintaining advanced standards of living. Apart from conversion efficiency, fuel cells have other aspects that make them attractive: Their conversion process is clean, they may cogenerate useful heat, and they can be used in a variety of fields of application.
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